magnetism as seen with x rays - spallation neutron sourceneutrons.ornl.gov/sites/default/files/elke...
TRANSCRIPT
![Page 1: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/1.jpg)
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Magnetism as seen with X Rays
Elke ArenholzLawrence Berkeley National Laboratory
andDepartment of Material Science and Engineering, UC Berkeley
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+ Magnetic Materials Today
+ Magnetic Materials Characterization Wish List
+ Soft X-ray Absorption Spectroscopy – Basic concept and examples
+ X-ray magnetic circular dichroism (XMCD)
- Basic concepts
- Applications and examples
- Dynamics: X-Ray Ferromagnetic Resonance (XFMR)
+ X-Ray Linear Dichroism and X-ray Magnetic Linear Dichroism (XLD and XMLD)
+ Magnetic Imaging using soft X-rays
+ Ultrafast dynamics
What to expect:
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Magnetic Materials Today
Magnetic materials for energy applications
Magnetic nanoparticles for biomedical andenvironmental applications
Magnetic thin films for
information storage and processing
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Permanent and Hard Magnetic Materials
Engineering magnetic anisotropy
on the atomic scale
Controlling grain and
domain structure on the micro-
and nanoscale
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Magnetic Nanoparticles
Tailoring magnetic nanoparticles for
environmentalapplications
Optimizing magnetic nanoparticles for biomedical applications
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GMR Read Head Sensor
Magnetic Thin Films
Magnetic domain structure on the nanometer scale
Unique magnetic phases at interfaces
Ultrafast magnetization
reversal dynamics
Magnetic couplingat interfaces
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Magnetic Materials Characterization Wish List
+ Sensitivity to ferromagnetic and antiferromagnetic order
+ Element specificity = distinguishing Fe, Co, Ni, …
+ Sensitivity to oxidation state = distinguishing Fe2+, Fe3+, …
+ Sensitivity to site symmetry, e.g. tetrahedral, Td; octahedral, Oh
+ Nanometer spatial resolution
+ Ultra-fast time resolution
Soft X-Ray Spectroscopy and Microscopy
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sample
inte
nsi
ty
wavelength, photon energy
inte
nsi
ty
wavelength, photon energy
Spectroscopy
Sample
Light/Photon Source
Monochromator
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SampleElectron Storage Ring Monochromator
Soft X-Ray Spectroscopy ( h 500-1000eV, 1-2nm)
770 780 790 8000.6
0.7
0.8
0.9
1.0
photon energy (eV)
tran
sm
itte
d i
nte
nsit
y I
t / I
0
EY
_T
M.o
pj
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10
770 780 790 8000
2
4
6
EY
_T
M.o
pj
ele
ctr
on
yie
ld I
e /
I0
photon energy (eV)
770 780 790 8000.6
0.7
0.8
0.9
1.0
photon energy (eV)
tran
sm
itte
d i
nte
nsit
y I
t / I
0
EY
_T
M.o
pj
Photonsabsorbed
Electronsgenerated
Electron yield: + Absorbed photons create core holes subsequently filled by Auger electron emission+ Auger electrons create low-energy secondary electron cascade through inelastic scattering+ Emitted electrons probability of Auger electron creation absorption probability
J. Stöhr, H.C. Siegmann,Magnetism (Springer)
X-Ray Absorption Detection Modes
mean free path 5nm
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10-20 nm layer thick films supported by substrates transparent to soft X rays
640 660
0.8
1.0
700 720 780 800 860 880
I t /
I0
photon energy (eV)
Fe
lum
inescence_B
L402_A
pr2
012.o
pj
Co
//////
////Ni
Mn//
Ru
MnIr
CoFe
Ru
NiFe
Ru
Soft X-Ray Absorption – Probing Depth
3nm
15nm
5nm
3nm
15nm
15nm
Element 10eV below L3
1/ [nm]
at L3
1/ [nm]
40 eV above L3
1/ [nm]
Fe 550 17 85
Co 550 17 85
Ni 625 24 85
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0.8
1.0
0.8
1.0
0.8
1.0
0.8
1.0
Mn NiCoe
lectr
on
yie
ld (
arb
. u
nit
s)
I t /
I0
Fe
640 650 660
0.9
1.0
photon energy (eV)
lum
inescence_B
L402_A
pr2
012.o
pj
710 720
1.0
1.1
photon energy (eV)
780 790
0.9
1.0
photon energy (eV)
850 860 870
1.0
1.2
1.4
photon energy (eV)
Ru
MnIr
CoFe
Ru
NiFe
Ru
e
3nm
15nm
5nm
3nm
15nm
15nm
X-Ray Absorption Detection Modes and Probing Depth
+ Electron sample depth: 2-5 nm in Fe, Co, Ni 60% of the electron yield originates form the topmost 2-5 nm
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Experimental Concept:Monitor reduction in X-ray flux transmitted through sample as function of photon energy
Charge state of absorber Fe2+, Fe3+
Symmetry of lattice site of absorber: Oh, Td
Sensitive to magnetic order
Core level Atomic species of absorber Fe, Co, Ni, …. 2p3/2 L3
2p1/2 L2
Valence states
Absorption probability: X-ray energy, X-ray polarization,experimental geometry
X-Ray Absorption Fundamentals
E
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Experimental Concept:Monitor reduction in X-ray flux transmitted through sample as function of photon energy
Charge state of absorber Fe2+, Fe3+
Symmetry of lattice site of absorber: Oh, Td
Sensitive to magnetic order
Core level Atomic species of absorber Fe, Co, Ni, …. 2p3/2 L3
2p1/2 L2
Valence states
Absorption probability: X-ray energy, X-ray polarization,experimental geometry
X-Ray Absorption Fundamentals
E
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core level2p3/2 L3
2p1/2 L2
valence states
‘White Line’ Intensity
Fe
Intensity of L3,2 resonances is proportional to number of d states above the Fermi level, i.e. number of holes in the d band.
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core level2p3/2 L3
2p1/2 L2
valence states
‘White Line’ Intensity
Fe
Intensity of L3,2 resonances is proportional to number of d states above the Fermi level, i.e. number of holes in the d band.
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2p3/2 L3
2p1/2 L2
valence states
‘White Line’ Intensity
Co
core level
Intensity of L3,2 resonances is proportional to number of d states above the Fermi level, i.e. number of holes in the d band.
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2p3/2 L3
2p1/2 L2
valence states
‘White Line’ Intensity
Ni
core level
Intensity of L3,2 resonances is proportional to number of d states above the Fermi level, i.e. number of holes in the d band.
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2p3/2 L3
2p1/2 L2
valence states
Intensity of L3,2 resonances is proportional to number of d states above the Fermi level, i.e. number of holes in the d band.
‘White Line’ Intensity
Cu
core level
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Experimental Concept:Monitor reduction in X-ray flux transmitted through sample as function of photon energy
Charge state of absorber Fe2+, Fe3+, … Symmetry of lattice site of absorber: Oh, Td
Sensitive to magnetic order
Core level Atomic species of absorber Fe, Co, Ni, …. 2p3/2 L3
2p1/2 L2
Valence states
Absorption probability: X-ray energy, X-ray polarization,experimental geometry
X-Ray Absorption Fundamentals
E
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N. Telling et al.,Appl. Phys. Lett. 95, 163701 (2009)
Influence of the charge state of the absorber
J.-S. Kang et al., Phys. Rev. B 77, 035121 (2008)
X-ray Absorption – Valence State
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J. Stöhr, H.C. Siegmann,Magnetism (Springer)
X-Ray Absorption – Configuration Model
Ni2+ in NiO: 2p6 3d8 → 2p5 3d9
Configuration model, e.g. L edge absorption :
+ Excited from ground/initial state configuration, 2p63d8
to exited/final state configuration, 2p53d9
+ Omission of all full subshells (spherical symmetric)
+ Takes into account correlation effects in the ground state as well as in the excited state
+ Leads to multiplet effects/structure
http://www.anorg.chem.uu.nl/CTM4XAS/ 2S+1L
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Experimental Concept:Monitor reduction in X-ray flux transmitted through sample as function of photon energy
Charge state of absorber Fe2+, Fe3+
Symmetry of lattice site of absorber: Oh, Td
Sensitive to magnetic order
Core level Atomic species of absorber Fe, Co, Ni, …. 2p3/2 L3
2p1/2 L2
Valence states
Absorption probability: X-ray energy, X-ray polarization,experimental geometry
X-Ray Absorption Fundamentals
E
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455 460 465 470
PZ
T_X
A.o
pj
photon energy (eV)
XA
(arb
. u
nit
s)
PbZr0.2Ti0.8O2
Sensitivity To Site Symmetry: Ti4+ L3,2
+ Electric dipole transitions: d02p53d1
+ Crystal field splitting 10Dq acting on 3d orbitals:
Octahedral symmetry: e orbitals towards ligands higher energyt2 orbitals between ligands lower energy
Tetragonal symmetry:e orbitals b2 = dxy, e = dyz, dyz
t2 orbitals b1 = dx2y
2, a1 = d3z2r
2
J. Stöhr, H.C. Siegmann,Magnetism (Springer)
t2
e e
t2
3d orbitals
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x-
ray a
bs
orp
tio
n
TiO2
Oh
D2h G. Van der Laan
Phys. Rev. B 41, 12366 (1990)
Influence of lattice site symmetry at the absorber
X-Ray Absorption Lattice Symmetry
rutile
anatase
TiO2
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Experimental Concept:Monitor reduction in X-ray flux transmitted through sample as function of photon energy
Charge state of absorber Fe2+, Fe3+
Symmetry of lattice site of absorber: Oh, Td
Sensitive to magnetic order
Core level Atomic species of absorber Fe, Co, Ni, …. 2p3/2 L3
2p1/2 L2
Valence states
Absorption probability: X-ray energy, X-ray polarization,experimental geometry
X-Ray Absorption Fundamentals
E
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Experimental Concept:Monitor reduction in X-ray flux transmitted through sample as function of photon energy
Charge state of absorber Fe2+, Fe3+
Symmetry of lattice site of absorber: Oh, Td
Sensitive to magnetic order
Core level Atomic species of absorber Fe, Co, Ni, …. 2p3/2 L3
2p1/2 L2
Valence states
Absorption probability: X-ray energy, X-ray polarization,experimental geometry
X-Ray Absorption Fundamentals
E
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+ Magnetic moments in Fe, Co, Ni well described by Stoner model:d-bands containing up and down spins shifted relative to each other by exchange splitting
+ Spin-up and spin-down bands filled according to Fermi statistics
+ Magnetic moment |m| determined by difference in number of electrons in majority and minority bands
empty states,
“holes”
exchange
splitting
3d shell
spin-upspin-down
empty states,
“holes”
)n(nμ m|| mine
majeB
Stoner Model For Ferromagnetic Metals
J. Stöhr, H.C. Siegmann,Magnetism (Springer)
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Origin of X-ray Magnetic Circular Dichroism
2-Step Model for photoexcitation of electrons from 2p3/2, 2p1/2 to 3d states by absorption of circularly polarized X rays:
+ Transfer of angular momentum of incident circular polarized X rays to excited electrons (angular momentum conservation, selection rules)
+ Spin polarization of excited electrons opposite for incident X rays with opposite helicity.
+ Unequal spin-up and spin-down populations in exchange splitvalence shell acts as detector for spin of excited electrons.
3d
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+ Calculate transition probabilities from filled 2p3/2 and 2p1/2 states to empty states in d-bandfor circularly polarized X raysusing Fermi’s Golden Rule
Origin of X-ray Magnetic Circular Dichroism
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Origin of X-ray Magnetic Circular Dichroism
initial state |iinitial state energy i
final state |ffinal state energy f
+ Wave functions describe electronic and photon statesEnergies include electronic and photon energies
+ Calculate transitions probabilities Tif
considering photon as time-dependent perturbation,i.e. an electromagnetic (EM) field
ρ(εf ) = density of final states per unit energy
Tif Dimension [time−1]
Fermi’s Golden Rule
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+ Consider strong ferromagnet with one filled spin band: All spin down d states filled Spin up d states partially filled
+ This specific case:Only spin up electron excited
X-ray absorption of circularly polarized photons with angular momentum q = ±1 in units of ħ
Origin of X-ray Magnetic Circular Dichroism
↓
↓
↓
↓
J. Stöhr, H.C. Siegmann,Magnetism (Springer)
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Origin of X-ray Magnetic Circular Dichroism
q = +1 q = 0q = 1 q=1q=+1 q=0
L3
L2
50 30 10 30
L3: X rays with q = +/1 excite 62.5%/37.5% of the spin up electronsL2: X rays with q = +/1 excite 25%/75% of the spin up electrons
J. Stöhr, H.C. Siegmann,Magnetism (Springer)
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Origin of X-ray Magnetic Circular Dichroism
↓
↓
↓
↓
J. Stöhr, H.C. Siegmann,Magnetism (Springer)
Taking into account 2x higher population of 2p3/2 state as compared to 2p1/2 state:
Identical magnitude XMCD at L3 and L2 with opposite sign
= 25% = -50%
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Magnitude of XMCD depends on+ expectation value of 3d
magnetic moment+ degree of circular photon
polarization, Pcirc
+ geometry
IXMCD = I I
0.0
0.5
1.0
770 780 790 800
-0.4
-0.2
0.0
photon energy (eV)
XA
(a
rb.
un
its
)
FeC
o_G
aA
s_X
MC
D.o
pj
XM
CD
(arb
. u
nit
s)
L3L2
Co
X-Ray Magnetic Circular Dichroism (XMCD)
![Page 36: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/36.jpg)
36
0.0
0.5
1.0
700 710 720 730 780 790 800
-0.2
0.0
XA
(a
rb.
un
its
)
photon energy (eV)
XM
CD
(arb
. u
nit
s)
C
oF
e2O
4.o
pj
L3 Fe Co
L2
L3
L2
CoFe2O4
Fe2+,Oh
Fe3+, Oh
Fe3+, Td
Co2+
J. Stöhr, H.C. Siegmann,Magnetism (Springer)
H
circularlypolarized
+ XMCD provides magnetic information resolving elements Fe, Co, …valence states: Fe2+, Fe3+, …lattice sites: octahedral, Oh, tetrahedral, Td,
X-Ray Magnetic Circular Dichroism (XMCD)
![Page 37: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/37.jpg)
37
+ Geobacter sulfurreducens bacteria form magnetite nanocrystals (15nm)via extracellular reduction of amorphous Fe(III)-bearing minerals
Magnetic Bionanospinels
Fe3O4
Co-ferrite-1 6 at% Co
Co-ferrite-2 23 at% Co
XM
CD
photon energy (eV)
V. Cocker et al.,
Eur. J. Mineral. 19, 707–716 (2007)2 0 +2
60
0
+60
H (T)
M (
em
u g
1)
Fe2+,Oh
Fe3+, Oh
Fe3+, Td
![Page 38: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/38.jpg)
38
V. Cocker et al.,
Eur. J. Mineral. 19, 707–716 (2007)2 0 +2
60
0
+60
H (T)
M (
em
u g
1)
Co2+ Oh
Magnetic Bionanospinels
+ Geobacter sulfurreducens bacteria form magnetite nanocrystals (15nm)via extracellular reduction of amorphous Fe(III)-bearing minerals
![Page 39: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/39.jpg)
39
+ Comparing XMCD spectra with model compounds and/or calculations Identifying magnetic phases
XA
, X
MC
D
Co metal
XA
XA
XMCD
XMCD
photon energy (eV)
Co2+
in CoFe2O
4
780 790 800
0
0
XA
, X
MC
D
Co_C
o2+
.opj
Co-doped TiO2X
MC
D (
arb
. un
its)
XA
(ar
b. u
nit
s)
Co-doped TiO2
dilute magnetic semiconductors
J.-Y. Kim et al., Phys. Rev. Lett. 90, 017401 (2003)
780 800790 810photon energy (eV)
![Page 40: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/40.jpg)
40
Cu
Co
Cu
Co
…
+ The element-specificity makes XMCD measurements an ideal tool to determine induced moments at interfaces between magnetic and non-magnetic elements.
Induced Moments At Co/Cu Interfaces
M. G. Samant et al.,Phys. Rev. Lett. 72, 1112 (1994)
![Page 41: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/41.jpg)
41
Mn L3,2
Co L3,2
XA
(a
rb.
un
its
)
630 640 650 660 770 780 790 800 810
XM
CD
(a
rb.
un
its
)
photon energy (eV)
x200
20 Å Co / 200 Å Ir20Mn80
+ Weak Mn XMCD signal
Uncompensated Mn at Co/IrMn interface
+ Same sign of XMCD signal for Co and Mn
Parallel coupling of Co and Mnmoments
+ Nominal thickness of uncompensated interface moments: (0.50.1)ML
IrMn
Co
Magnetic Interfaces
H. Ohldag et al.,
Phys. Rev. Lett. 91, 017203 (2003)
FM
AFM
H = +/-0.5T
![Page 42: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/42.jpg)
42
705 710 715 720 725
-0.50
-0.25
0.00
0.25
710 712-0.02
0.00
0.02
0.0 0.2 0.4 0.6
-0.50
-0.25
0.00
0.0
0.5
1.0
X
MC
D (
arb
. u
nit
s)
photon energy (eV)
photon energy (eV)
XA
(a
rb.
un
its
)
XM
CD
(a
rb.
un
its
)
Fe L
3 X
MC
D
(arb
. u
nit
s)
x
0.0 0.2 0.4 0.6
-0.50
-0.25
0.00
Fe
L3 (
eV
)
x
Band Filling In GaxFe1−x
+ Fe majority-spin filled for x=0.3+ x 0.3: Fe moment decrease strongly,
Formation of D03 precipitates
J. Stöhr, H.C. Siegmann,Magnetism (Springer)
GaxFe1−x
Fe L3,2
E. Arenholz et al.,Phys. Rev. B 82, 180405 ( 2010)
![Page 43: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/43.jpg)
43
Composition Dependence of Fe moment in Fe1-xMnx
Drop of magnetic moment in bcc Fe1-xMnx, i.e. independent of structural transition
![Page 44: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/44.jpg)
44
A < 0
B > 0
+ Theoretically derived sum rules correlate XMCD spectra with spin and orbital moment providing unique tool for studying magnetic materials.
mS = B–A + 2B / C
mL = –2BA + B / 3CNh = IL3 + IL2 /C
Sum Rules
J. Stöhr, H.C. Siegmann,Magnetism (Springer)
![Page 45: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/45.jpg)
45
+ Strong variation of orbital and spin magnetic moment observable as change in relative L3 and L2 intensity in XMCD spectrum.
+ Co atoms and nanoparticles on Pt have enhanced orbital moments up to 1.1 B
P. Gambardella et al.,Science 300, 1130 (2003)
Orbital Moment Of Co Nanoparticles
![Page 46: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/46.jpg)
46
Element-specific Magnetization Reversal
Co L3,2
+/- circ. pol.
H = -0.5T
X
A (
arb
. u
nit
s)
780 800
0
I+ -
I- (
arb
. u
nit
s)
photon energy (eV)
+ Monitoring field dependence of XMCD Element-specific information on magnetization reversal in complex magnetic
nanostructures.
![Page 47: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/47.jpg)
47
XA
(arb
. u
nit
s)
Co L3,2
+/- circ. pol.
H = +0.5T
780 800
0
I+ -
I- (
arb
. u
nit
s)
photon energy (eV)
Co L3,2
+/- circ. pol.
H = -0.5T
X
A (
arb
. u
nit
s)
780 800
0
I+ -
I- (
arb
. u
nit
s)
photon energy (eV)
Element-specific Magnetization Reversal
+ Monitoring field dependence of XMCD Element-specific information on magnetization reversal in complex magnetic
nanostructures.
![Page 48: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/48.jpg)
48
-0.4 -0.2 0.0 0.2 0.4
0
XM
CD
magnetic field (T)
+ Monitoring field dependence of XMCD Element-specific information on magnetization reversal in complex magnetic
nanostructures.
Co L3,2
+/- circ. pol.
H = -0.5T
X
A (
arb
. u
nit
s)
780 800
0
I+ -
I- (
arb
. u
nit
s)
photon energy (eV)
XA
(arb
. u
nit
s)
Co L3,2
+/- circ. pol.
H = +0.5T
780 800
0
I+ -
I- (
arb
. u
nit
s)
photon energy (eV)
Element-specific Magnetization Reversal
![Page 49: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/49.jpg)
49
x3
H=+0.2 TH=-0.2 T
XA
(a
rb.
un
its
)
700 750 800 850
0
XM
CD
photon energy (eV)
Fe
Co
Ni
5 ML Co
8,10 ML Fe
18 ML Ni
-40 -20 0 20 40
-10
-5
0
5
10
XM
CD
(%
)
field (mT)
NiFeCo
8 ML Fe
Element-specific Magnetization Reversal
![Page 50: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/50.jpg)
50
-40 -20 0 20 40
-10
-5
0
5
10
XM
CD
(%
)
field (mT)
NiFeCo
x3
H=+0.2 TH=-0.2 T
XA
(a
rb.
un
its
)
700 750 800 850
0
XM
CD
photon energy (eV)
Fe
Co
Ni
8 ML Fe
5 ML Co
8,10 ML Fe
18 ML Ni
-200 -100 0 100 200-10
-5
0
5
10
XM
CD
(%
)field (mT)
NiFeCo
10 ML Fe
Element-specific Magnetization Reversal
![Page 51: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/51.jpg)
51
X-Ray Ferromagnetic Resonance
+ XMCD is the difference in X-ray absorption between antiparallel and parallel orientation of magnetic moment and photon spin.
+ The XMCD magnitude reflects the magnetic moment aligned parallel to the X ray beam.
0.0
0.5
1.0
770 780 790 800
-0.4
-0.2
0.0
photon energy (eV)
XA
(a
rb.
un
its
)
FeC
o_G
aA
s_X
MC
D.o
pj
XM
CD
(arb
. u
nit
s)
L3L2
Co
H
circularlypolarized
![Page 52: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/52.jpg)
52
0.0
0.5
1.0
770 780 790 800
-0.4
-0.2
0.0
photon energy (eV)
XA
(a
rb.
un
its
)
FeC
o_G
aA
s_X
MC
D.o
pj
XM
CD
(arb
. u
nit
s)
L3L2
Co
H
circularlypolarized
M(t)
+ In fact: Magnetic moments are not fully aligned with applied fields but precess around them.
X-Ray Ferromagnetic Resonance
![Page 53: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/53.jpg)
53
0.0
0.5
1.0
770 780 790 800
-0.4
-0.2
0.0
photon energy (eV)
XA
(a
rb.
un
its
)
FeC
o_G
aA
s_X
MC
D.o
pj
XM
CD
(arb
. u
nit
s)
L3L2
Co
H
circularlypolarized
M(t)
H
M x H
+ In fact: Magnetic moments are not fully aligned with applied fields but precess around them.
+ Is it possible to measure the pression of magnetic moments making use of the pulsed nature of synchrotron radiation and XMCD? (!)
X-Ray Ferromagnetic Resonance
![Page 54: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/54.jpg)
54
Pulsed nature of synchrotron radiationExample: Advanced Light Source
bunch spacing
Pulse length 70 ps
+ 256-320 bunches for 500mA beam current
+ Bunch spacing: 2 ns (500MHz)
+ Pulse length 70ps
X-Ray Ferromagnetic Resonance
![Page 55: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/55.jpg)
55
Dynamic XMCD measurement, i.e. synchronize X-ray pulses with FMR precession
M(t)
HB
X-ray pulses
microwave
driving field
~70 ps2 ns
Mz(t)
X-ray pulse repetition signal, ~500 MHz
f = n500 MHz
X-Ray Ferromagnetic Resonance
![Page 56: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/56.jpg)
56
0 200 400 600 800 1000-4
-2
0
2
4
XM
CD
(arb
. units)
Microwave delay (ps)
M
X-rays
M
M(t)
Static XMCD Dynamic XMCD
0.0
0.5
1.0
770 780 790 800
-0.4
-0.2
0.0
photon energy (eV)
XA
(a
rb.
un
its
)
FeC
o_G
aA
s_X
MC
D.o
pj
XM
CD
(arb
. u
nit
s)
L3
L2
Co
X-Ray Ferromagnetic Resonance
![Page 57: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/57.jpg)
57
+ Precession is resonantly excited in the NiFe layer with an 4 GHz RF field.
+ The resonance field of the CO layer is higher, i.e. no precession is excited in the Co layer.
+ Precession in Py, Cu75Mn25, and Co layers are probed by XMCD using left- and right-circularly polarized X-rays at Ni, Mn, and Co edges, respectively.
+ The Cu75Mn25 spin precession is a direct indicator of the AC spin current through the structure.
X-Ray Ferromagnetic Resonance
![Page 58: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/58.jpg)
58
X-Ray Linear Dichroism:
+ Difference in X-ray absorption for different linear polarization direction relative to crystalline and/or spin axis.
+ Due to the anisotropic charge distribution about the absorbing atom caused by bonding and/or magnetic order.
+ “Search Light Effect”: X-ray absorption of linear polarized X rays proportional to density of empty valence states in direction of electric field vector E.
Cu
O
photon energy (eV)920 940 960
La1.85Sr0.15CuO4
L2
Cu
XA
(ar
b. u
nit
s)
L3
C. T. Chen et al. PRL 68, 2543 (1992)
X-Ray Linear Dichroism
E
![Page 59: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/59.jpg)
59
Pb2+ O2 Ti4+, Zr4+
+
ferroelectric polarization
+ Spontaneous electric polarization due to off-center shift of Ti4+, Zr4+ associated with tetragonal distortion linear dichroism
+ Reversing ferroelectric polarization changes XA Change in tetragonal distortion
0.0
0.5
1.0
455 460 465 470
-0.05
0.00
XA
(arb
. u
nit
s)
dif
fere
nc
e
(arb
. u
nit
s)
// //
0.0
0.5
1.0
XA
(arb
. u
nit
s)
-0.2
0.0
0.2
photon energy (eV)
dif
fere
nc
e
(arb
. u
nit
s)
////
////
Structural Changes In PbZr0.2Ti0.8O3
as grown
reversed
t2
e et2
E. Arenholz et al.,Phys. Rev. B 82, 140103 (2010)
![Page 60: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/60.jpg)
60
→→
+ IXMLD = I|| I m 2 , m 2 = expectation value of square of atomic magnetic moment
+ XMLD allows investigating ferri- and ferromagnets as well as antiferromagnets
+ XMLD spectral shape and angular dependence are determined by magnetic order and lattice symmetry
Isotropic d electron charge density No polarization dependence
Magnetically aligned system Spin-orbit coupling distorts
charge density Polarization dependence
SL
L3
Fe Co
L3L2
CoFe2O4
L2
= 0
= 45H
H
X-Ray Magnetic Linear Dichroism
[001]0.0
0.5
1.0
XM
LD
(arb
. u
nit
s)
XA
(arb
. u
nit
s)
Co
Fe
2O
4_
11
0_
Se
pt.o
pj
-0.02
0.00
0.02
photon energy (eV)
700 710 720 730 780 790 800
//
//
//
![Page 61: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/61.jpg)
61
→
0.0
0.5
1.0
-0.05
0.00
0.05
850 855 860 865 870 875
Co
NiO
_4
.0.2
_N
i_X
ML
D.o
pj
XA
(a
rb.
un
its
)X
ML
D (
arb
. u
nit
s)
photon energy (eV)
→
+ IXMLD = I|| I m 2 , m 2 = expectation value of square of atomic magnetic moment
+ XMLD allows investigating ferri- and ferromagnets as well as antiferromagnets
+ XMLD spectral shape and angular dependence are determined by magnetic order and lattice symmetry
L3
L3
Isotropic d electron charge density No polarization dependence
Magnetically aligned system Spin-orbit coupling distorts
charge density Polarization dependence
antiferromagnetic NiO
= 0
S
= 45
L
[001]
[001]
X-Ray Magnetic Linear Dichroism
![Page 62: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/62.jpg)
62
LSFO
640 650-0.2
0.0
0.0
0.5
1.0
XA
(a
rb.
un
its
)
photon energy (eV)
XM
CD
(arb
. u
nit
s)
0.0
0.5
1.0
710 720
-0.2
0.0
0.2
XA
(arb
. u
nit
s)
expt. calc.
photon energy (eV)
XM
LD
(arb
. u
nit
s)
0.0
0.5
1.0
710 720
-0.1
0.0
0.1
XA
(a
rb.
un
its
)
XM
LD
(arb
. u
nit
s)
photon energy (eV)
Magnetic Coupling At Interfaces
HMn XMCD
Fe XMLD
H
Perpendicular coupling
at LSMO/LSFO interface
LSMO
La0.7Sr0.3MnO3 (LSMO)ferromagnet
La0.7Sr0.3FeO3 (LSFO)antiferromagnet
H
0.0
0.5
1.0
0.0
0.5
1.0
0 100 200 300 4000.0
0.5
1.0
Fe
L3,2 X
ML
D (a
rb. u
nits
)
Mn
L3,2 X
MC
D
(arb
. u
nit
s)
Fe
L3,2 X
ML
D
(a
rb.
un
its
)
temperature (K)
E. Arenholz et al.,Appl. Phys. Lett. 94, 072503 (2009)
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63
770 780 790 850 860 870
0.0
0.5
1.0L3
L2
L2
Ni
Co
CoN
iO_6.3
.1.o
pj
X
MC
D,
XA
(a
rb.
un
its
)
photon energy (eV)
Co/NiO
x50
L3
A. Scholl et al.,
Phys. Rev. Lett. 92, 247201 (2004)
Co
NiO
1
2
868 870 872
-0.2
0.0
photon energy (eV)
XM
LD
(arb
. u
nit
s)
NiO
Co/NiO
XA
(arb
. u
nit
s)
0.0 0.2 0.4 0.6
0.9
1.0
1.1
1.2
Ni
L2 r
ati
o
applied field (T)
EH E||H
0o
10o
20o
30o
40o
50o
wa
ll an
gle
H
-0.5 0.0 0.5
-10
0
10
Co
XM
CD
(a
rb.
un
its
)
field (T)
NiO
Co
H
Planar Domain Wall
FM
AFM H
![Page 64: Magnetism as seen with X Rays - Spallation Neutron Sourceneutrons.ornl.gov/sites/default/files/Elke Arenholz Presentation.pdf · Origin of X-ray Magnetic Circular Dichroism 2-Step](https://reader033.vdocuments.mx/reader033/viewer/2022060506/5f1f24ba6143196fc579486c/html5/thumbnails/64.jpg)
64
Magnetic Microscopy
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65
10-50 nm spatial resolutionJ. Stöhr, H.C. Siegmann,Magnetism (Springer)
Magnetic Microscopy
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66
780 790 800
0.0
0.5
1.0
Co/NiO(001)
photon energy (eV)
XM
CD
, X
A (
arb
. u
nit
s)
070727_C
o_X
MC
D.o
pj
i070725_046_047_d
iv.jp
g
A / B
Imaging Magnetic Domains Using X-Rays
i070725_049_050_d
iv.jp
g
A / B
A
i070725_046.jp
g
B
i070725_050.jp
g
left circ. right circ.
+ Images taken with left and right circularly polarized X-rays at photon energies with XMCD, i.e. Co L3 edge, provide magnetic contrast and domain images.
E. Arenholz et al.,
Appl. Phys. Lett. 93, 162506 (2008)
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67
Co XMCD
Ni XMLD
probing in-plane
5 m
5 m
X rays
+ Taking into account the geometry dependence of the Ni XMLD signal
Perpendicular coupling of Co and NiO moments at the interface.
Magnetic Coupling At Co/NiO Interface
E. Arenholz et al.,
Appl. Phys. Lett. 93, 162506 (2008)
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68
+ First direct observation of vortex state in antiferromagnetic CoO and NiO disks in Fe/CoO and Fe/NiO bilayers using XMCD and XMLD.
+ Two types of AFM vortices:- conventional curling vortex
as in ferromagnets- divergent vortex,
forbidden in ferromagnets- thickness dependence of
magnetic interface coupling
J. Wu et al.,
Nature Phys. 7, 303 (2011)
divergent vortexconventional curling vortex
Magnetic Vortices
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69
Q. He et al., Nature Comm. 2, 225 (2011)
2m
2m
+ BiFeO3 – multiferroic = ferroelectric + antiferromagnetic+ Compressive strain on rhombohedral phase (R-phase)
induced by substrate tetragonal-like phase (T-phase) + Partial relaxation of epitaxial strain Formation of a nanoscale mixture of T- and R-phases
AFM
RT
AFM
Nanoscale Magnetic Phases
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70
Q. He et al.,
Nature Comm. 2, 225 (2011)
Nanoscale Magnetic Phases
XMCD PEEM
+ Highly distorted R-phase is the source of enhanced magnetic moment in the XMCD image.
2m
2m
AFM PFM
XMCD-PEEM
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71
el-splat-sp
el-lat
Ultrafast Magnetism
Spin-lattice relaxation time
Electron-phonon relaxation time
Electron-spinrelaxation time
+ Energy reservoirs in a ferromagnetic metal
+ Deposition of energy in one reservoir
Non-equilibrium distribution and subsequent relation through energy and angular momentum exchange
J. Stöhr, H.C. Siegmann,Magnetism (Springer)
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72
C. Boeglin, et al., Nature 465, 458 (2010)
+ Orbital (L) and spin (S) magnetic moments can change with total angular momentum is conserved.
+ Efficient transfer between L and S through spin–orbit interaction in solids
+ Transfer between L and S occurs on fs timescales.
+ Co0.5Pt0.5 with perpendicularmagnetic anisotropy
+ 60 fs optical laser pulses change magnetization
+ Dynamics probed with XMCD using 120fs X-ray pulses
+ Linear relation connects Co L3 and L2 XMCD with Lz and Sz using sum rules
Co0.5Pt0.5
Ultrafast Dynamics Of Spin And Orbital Moments
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73
+ Thermalization: Faster decrease of orbital moment
+ Theory: Orbital magnetic moment strongly correlated with magnetocrystalline anisotropy
+ Reduction in orbital moment Reduction in magnetocrystalline anisotropy
+ Typically observed at elevated temperatures in static measurements as well
C. Boeglin, et al., Nature 465, 458 (2010)
el-splat-sp
el-lat
Spin-lattice relaxation time
Electron-phonon relaxation time
Electron-spinrelaxation time
Ultrafast Dynamics Of Spin And Orbital Moments
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J. Stöhr, H.C. SiegmannMagnetism From Fundamentals to Nanoscale DynamicsSpringer
References And Further Reading